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  4. Crystal structure optimisation using an auxiliary equation of state
 
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Crystal structure optimisation using an auxiliary equation of state
File(s)
1.4934716.pdf (4.56 MB)
Published version
Author(s)
Jackson, AJ
Skelton, JM
Hendon, CH
Butler, KT
Walsh, A
Type
Journal Article
Abstract
Standard procedures for local crystal-structure optimisation involve numerous energy and force calculations. It is common to calculate an energy–volume curve, fitting an equation of state around the equilibrium cell volume. This is a computationally intensive process, in particular, for low-symmetry crystal structures where each isochoric optimisation involves energy minimisation over many degrees of freedom. Such procedures can be prohibitive for non-local exchange-correlation functionals or other “beyond” density functional theory electronic structure techniques, particularly where analytical gradients are not available. We present a simple approach for efficient optimisation of crystal structures based on a known equation of state. The equilibrium volume can be predicted from one single-point calculation and refined with successive calculations if required. The approach is validated for PbS, PbTe, ZnS, and ZnTe using nine density functionals and applied to the quaternary semiconductor Cu2ZnSnS4 and the magnetic metal-organic framework HKUST-1.
Date Issued
2015-11-09
Date Acceptance
2015-10-13
Citation
Journal of Chemical Physics, 2015, 143 (18)
URI
http://hdl.handle.net/10044/1/41655
DOI
https://www.dx.doi.org/10.1063/1.4934716
ISSN
1089-7690
Publisher
AIP Publishing
Journal / Book Title
Journal of Chemical Physics
Volume
143
Issue
18
Copyright Statement
© 2015 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License.
License URL
http://creativecommons.org/licenses/by/4.0/
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Physics, Atomic, Molecular & Chemical
Chemistry
Physics
GENERALIZED GRADIENT APPROXIMATION
DENSITY-FUNCTIONAL APPROXIMATIONS
METAL-ORGANIC FRAMEWORKS
AUGMENTED-WAVE METHOD
MOLECULAR-DYNAMICS
SOLAR-CELLS
ENERGY
EXCHANGE
DIFFRACTION
CU2ZNSNS4
Chemical Physics
02 Physical Sciences
03 Chemical Sciences
09 Engineering
Publication Status
Published
Article Number
184101
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